United States

Abstract Body: Recently, α-Ga2O3 have been attracting great attentions as an ultra-wide bandgap semiconductor. However, the reason why meta-stable α-Ga2O3, which was originally synthesized at a pressure of 44 kbar and at a temperature of 1000 °C [1], is grown at around 500 °C under atmosphere by mist chemical vapor deposition (CVD) has not been elucidated yet. In this study, in order to analyze the growth mechanisms of mist CVD-grown α-Ga2O3, we investigated the growth processes at the initial stage. α-Ga2O3 with thickness (t) of 2.3, 4.7, 7.8, and 30 nm were grown on (0001) sapphire by the mist CVD method. The four samples were investigated by atomic force micrograph (AFM), transmission electron micrograph (TEM), and X-ray diffraction reciprocal space mapping (XRD RSM). High resolution (HR-) TEM images at the interface viewed along the [11-20] axis indicates that α-Ga2O3 is pseudomophically grown on sapphire for t=2.3 nm, however, relaxed for t=4.7, 7.8, and 30 nm. Therefore, we found that the critical thickness of mist CVD-grown α-Ga2O3 on (0001) sapphire is 2.3-4.7 nm. In addition, for t=4.7, 7.8, and 30 nm, α-Ga2O3 was successfully grown even after the lattice relaxation. In TEM images under two-beam diffraction condition of g=10-10 viewed along the [11-20] , dark and bright regions periodically introduced in the film near the interface are seen, but not of g=0001, for t=4.7, 7.8, and 30 nm. Thus, it is considered that regions strained along in-plane direction or/and misfit dislocations with the Burger’s vector parallel to the interface are periodically introduced near the interface after the α-Ga2O3 film relaxes. From the electron diffraction patterns and XRD RSM, it is confirmed that the films of t=4.7, 7.8, and 30 nm keep α-phase even after the lattice relaxation. XRD RSM also indicates that relaxation ratio gradually increases as the film thickness increases; for t=30 nm, the film is almost free standing. We also calculated the critical thickness based on the force-balance model and obtained the value of ~4.2 nm, which is consistent to the prediction (2.3-4.7 nm) derived from the HR-TEM. From the above coincidence, it is considered that the relaxation of mist CVD-grown α-Ga2O3 is caused by dislocations. On the other hand, by MBE, PLD, and MOCVD previously reported, the lattice relaxation is caused by phase transition from α to β [2,3], that is, the frustration of taking the α-phase causes the lattice relaxation so that the crystal structure changes from α to β. The lattice relaxation processes by mist CVD are different from those by other growth methods. This may be attributed to the low temperature growth and the association of water in the growth atmosphere. We will discuss the mechanism in more detail at the conference. [1] J. P. Remeika et al., Appl. Phys. Lett. 8, 87 (1966). [2] R. Schewski et al., Appl. Phys. Express 8, 011101 (2015). [3] Z. Cheng et al., Appl. Phys. Lett. 111, 162104 (2017).

EMC 2021

On the Initial Growth Mechanisms of α-Phase Ga2O3 on c-Plane Sapphire by Mist CVD

crystal growth

mist cvd

meta-stable

gallium oxide

thin film

The Electronic Materials Conference (EMC) is the premier annual forum on the preparation, characterization and use of electronic materials. This year’s event will feature a plenary session, topical sessions, a poster session and more.

EMC is coordinated with the Device Research Conference (DRC), which will be held during the same week, from June 20-23. This recognizes the strong interaction between device and electronic materials research and provides fruitful exchange of information between attendees of both Conferences.

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technical paper

Abstract Body: Graphene plasmonic resonances have been broadly studied in the terahertz and mid-infrared (MIR) ranges because of their electrical tunability and large confinement factors, which can enable dramatic enhancement of light-matter interactions, among other optoelectrical applications. Plasmonic resonances occur in graphene when it is patterned into nanostructures (e.g. ribbons) which confine the graphene plasmons and enables coupling to free-space radiation. For nanostructures with dimensions greater than 15 nanometers, the characteristic scaling laws of the graphene plasmons are well approximated by the local model of graphene’s conductivity. However, we experimentally demonstrate that those scaling laws change for structures smaller than 15 nanometers due to non-local and quantum effects in the graphene. Those changes blue-shift the frequencies of the graphene plasmons, pushing their operational range from the MIR into the short-wave-infrared (SWIR). We realize these effects in centimeter-scale arrays of graphene nanoribbons as narrow as 12 nanometers that are created using a novel, bottom-up block copolymer lithography method. The devices we create exhibit tunable plasmonic resonances at wavelength as short as 2.2 μm, almost double the energy of the previous experimental works. Furthermore, the confinement factors of our resonators reach 137 ± 25, which is amongst the largest reported in literature for any type of 2D optical resonator. The combined SWIR response and large confinement factors coupled to a scalable and efficient fabrication method makes these graphene nanostructures an attractive platform to explore next-generation optoelectrical devices and strongly enhanced spontaneous emission in the SWIR.

Large-Area Arrays of Short-Wave-Infrared Graphene Plasmonic Resonators Exhibiting Strong Non-Local and Electron Quantization Effects

Abstract Body: Transition metal dichalcogenide (TMD) semiconductors are layered van der Walls materials that exhibit exceptional optoelectronic properties in monolayer form. Their atomically thin nature and reduced long-range dielectric screening make them ideal systems in which to study many-body electronic states. Notably, excitonic many-body phenomena govern the light-matter interactions in TMD semiconductors and open up new possibilities for novel optoelectronic devices, including new classes of quantum light sources. Thus, understanding the rich suite of many-body phenomena in these systems is motivated by potential applications in on-chip optoelectronics and by the insights that can be gained into the fundamental interactions that govern TMD material properties. Here, the dynamics of several higher-order excitons including trions, biexcitons, and charged biexcitons in monolayer-WSe2 are probed using temperature-, energy-, and power-dependent time-resolved optical spectroscopy. We find that the formation of multiexciton complexes is enhanced by increasing the optical excitation energy for a given density. This enhancement is attributed to formation from an electron-hole plasma which generates 200% more multiexcitons than a lower-energy exciton gas. We further find that the multiexciton enhancement is robust over many samples and diminished with increasing temperature. These studies reveal a complex interplay between the multiexcitons and single-excitons that depends on both the density and excitation energy of the initial exciton population and open new doors to a number of applications such as entangle photon pair production and lasing, highlighting the importance of understanding the formation and relaxation dynamics of the rich manifold of excitons in order to leverage 2D semiconductors for advanced technologies.

Enhanced Multiexciton Formation by an Electron-Hole Plasma in 2D Semiconductors

Abstract Body: Semiconducting two-dimensional (2D) materials possess intriguing optoelectronic properties owing to the unique layered confined structure, such as strong light-matter interaction and large exciton binding energies. Especially, their excitonic binding energies far exceeding thermal energy will allow for room-temperature optoelectronic applications, such as excitonic computing applications and optical interconnects. It is therefore of significant importance to engineer excitonic properties and dynamics. The most widely used approaches to modulate the semiconducting 2D materials' excitonic dynamics include modifying the dielectric environment,[1] applying strain,[2] and gate-tuning.[3] In this study, we study modulation of exciton dynamics in monolayer MoS2 via dielectric Coulomb engineering and local strain by correlating photoluminescence (PL) mapping and scanning probe microscopy characterization. A mixed-dimensional heterojunction (MDHJ) was fabricated consisting of monolayer MoS2, sub-μm 0-dimensional P(VDF-TrFE) copolymer islands, and hBN. An optical microscope image, AFM topography map, and side view schematic of the MDJS are showing in Figures 1a, 1b, and 1c, respectively. Photoluminescence (PL) maps were obtained; A and B exciton emissions were fitted to Gaussians for parameter extraction (Figure 2a and 2b) and correlated with the topography data (Figure 2c). A clear blueshift of A exciton emission energy was observed on 1L-MoS2 on P(VDF-TrFE) islands with respect to 1L-MoS2 on hBN (Figure 2b). MoS2 on the polymer islands (red scatter plot; draped over polymer islands) showed a noticeable blueshift of ~3 meV compared to that of planar MoS2 on hBN (blue scatter plot) (Figure 2c). The bandgap increase can be attributed to the band structure renormalization and binding energy decrease due to the strong dielectric screening of the P(VDF-TrFE) substrate (εr ≈ 13).[1] Effects of dielectric environment and local strain on excitonic dynamics were examined by analyzing the A and B exciton intensity ratio; a high A-to-B intensity ratio is a sign of low nonradiative recombination.[4] Regions of increased A/B ratio (up to 2x) correlate well with the P(VDF-TrFE) islands locations (Figure 3a). Suppressed B exciton from the MoS2/P(VDF-TrFE) region contributes to the majority of the A/B ratio enhancement. Moreover, the B intensity showed a negative correlation with height, suggesting that large substrate screening combined with higher strain from the morphology enhances the intravalley scattering from the B exciton state to the A exciton state (Figure 3b). The A and B exciton energy difference map (Figure 3c) demonstrates that in contact with P(VDF-TrFE), the spin-orbit coupling-induced valence band splitting reduces, which may lead to an increased intravalley scattering rate. The correlation of PL and topography map revealed that the substrate dielectric screening and local strain affect the exciton dynamics of monolayer MoS2. [1] A. Raja et al., "Coulomb engineering of the bandgap and excitons in two-dimensional materials," Nat. Commun., vol. 8, no. May, p. 15251, May 2017. [2] A. Castellanos-Gomez et al., "Local Strain Engineering in Atomically Thin MoS 2," Nano Lett., vol. 13, no. 11, pp. 5361–5366, Nov. 2013. [3] Z. Qiu et al., "Giant gate-tunable bandgap renormalization and excitonic effects in a 2D semiconductor," Sci. Adv., vol. 5, no. 7, p. eaaw2347, Jul. 2019. [4] K. M. McCreary, A. T. Hanbicki, S. V. Sivaram, and B. T. Jonker, "A- and B-exciton photoluminescence intensity ratio as a measure of sample quality for transition metal dichalcogenide monolayers," APL Mater., vol. 6, no. 11, p. 111106, Nov. 2018.

Dielectric Effects on Exciton Emission of MoS2/P(VDF-TrFE) Heterostructure—A Correlated Mapping Study

Abstract Body: Abstract The two-dimensional insulating material hexagonal boron nitride (h-BN) has attracted much attention for resistive switching applications, yet its performance needs to be improved. In this work we present our comprehensive study of the resistive switching behavior of monolayer h-BN films with different electrode materials. The h-BN monolayers and h-BN/graphene heterostructure are synthesized on Ni substrates using molecular beam epitaxy (MBE), then Ni and Al are deposited as top electrodes. Three types of resistive switching devices are fabricated, namely, the symmetric metal-insulator-metal (MIM) device with Ni/h-BN/Ni, asymmetric MIM devices with Al/h-BN/Ni, and metal-insulator-graphene devices with Ni/h-BN/graphene and Al/h-BN/graphene structures. The symmetric Ni/h-BN/Ni devices demonstrate a polarity independent bipolar resistive switching behavior, a good durance with up to 97 cycles at 100 mA compliance current, an average on/off window of 103, and a low set and reset voltage variability. The asymmetric Al/h-BN/Ni devices demonstrate polarity dependent set voltage, with the larger set voltage observed when positive bias is applied on Ni. The metal/h-BN/graphene devices demonstrate self-compliant current bipolar resistive switching. The formation of conductive filaments is attributed to the diffusion of metallic ions and trapped charges. Our work reveals the influence of electrodes on resistive switching devices and provide ways to control the resistive switching behavior of two-dimensional h-BN based devices.

Resistive Switching Properties of Single Layer h-BN Film with Different Electrodes

Abstract Body: Graphene microstructures have been shown to exhibit controllable directional electron emission when carrying a current under an accelerating electric field. Through Phonon-Assisted Electron Emission (PAEE), graphene microstructures demonstrate electron emission at electric field intensities and lattice temperatures below what would be expected for carbon to demonstrate field emission or thermionic emission, respectively. Furthermore, such emissions tend to be out of the plane of the graphene microstructure, giving some control of the directionality of the emission current even before being directed with an applied electric field Thus far, such arrangements have tended to involve structural dimensions in the range of a handful of μm, commonly with CVD transferred graphene, flakes, or carbon nanotubes, with applied fields that can get up to the order of hundreds of kV/cm, and emission currents rarely exceeding a few nA. Herein are some examples of the characteristics and tunable variables demonstrated by multiple graphene structures with some dimensions up to cm, in fields below 4 kV/cm, and producing >1 μA emission currents. Quasi-freestanding epitaxial graphene on a silicon carbide substrate offers several advantages compared to transferred graphene or unzipped nanotubes, including lower defect density, greater structural integrity, ease of handling, and compatibility with simple photolithography fabrication techniques. The devices presented here were fabricated with a low-cost, wafer scalable, single-photomask process that does not require material transfer to a secondary substrate and is easily tailored to create variations in design parameters, which allowed multiple batches of devices to be rapidly manufactured with precise variations for the purpose of performance testing. The devices exhibited recognizable patterns of emission that seem to be influenced by several factors including, but not limited to shape and orientation, resistivity, input power, active time and on/off cycling frequency, device and substrate temperature, applied electric field, and both total device length and width dimensions (relative to current flow). Emission current seemed to show its most substantial dependence on input power, sometimes as much as doubling output with only a 25% increase in input; it is unknown if this relation holds for devices that vary other parameters alongside power input, necessitating further testing. The devices strongly imply a direct relationship between emission current density and device and substrate temperature, as some devices produced current outputs that exceeded measuring limits. Devices with larger dimensions also tended to produce more significant emission currents. However, the trends between increasing length and increasing width were not symmetrical: increasing device length (along the path of the input current) showed a stronger corresponding increase in output relative to % change in dimension than did changes in device width, and preliminary simulation results indicate both factors to have a roughly linear positive trend. While a general trend of larger dimensions and higher applied power levels tended to accompany higher emission currents, the output variations that may be attributed to other variables will allow for a broader range of device optimization parameters or tailoring of devices for specific purposes. Graphene microstructure electron sources may provide a means for device implementation in a 2D heterostructure environment or as a vehicle for further miniaturization of constructs requiring controllable electron emissions, such as electron microscopy or X-ray generation.

Characteristics and Tunability of Electron Emission Sources from Quasi-Freestanding Epitaxial Graphene Microstructures

Abstract Body: For the last few decades, most of the advancement in electronic and optoelectronic devices have been relying on our ability to integrate dissimilar materials having different lattice constants. By combining multiple different materials to form a heterostructure, we could engineer a particular band structure for a specific purpose. Nowadays the advancement on the integration technology is also motivated by the rapidly-growing field of Si photonics which requires integration of advanced non-Si infrared (IR) devices into the Si platform. However, to grow such devices on Si, one needs to address crystallographic challenges associated with high threading dislocations density caused by lattice mismatch. We have developed a novel materials integration technique, called metal-catalyzed lateral epitaxy, that has showed promising results in the Ge on Si system which has a 4% lattice mismatch. This technique uses a metal catalyst to control the growth location and a PECVD-grown capping layer to ensure growth laterally. The lateral growth is dictated by the vapor-liquid-solid mechanism which has shown a promising potential in suppressing the nucleation of threading dislocations by the extension of misfit dislocations. The main advantages of this technique over others are that it is wafer-scale, grown directly on the Si substrate, and allows direct electrical connection of the grown films to the substrate. In this talk, recent results of our systematic studies on the kinetics and the mechanism of this unique integration technique will be presented based on the heteroepitaxy of Ge-Si and InP-Si systems. Both are crucial heterostructures in Si photonics for high-performance IR photodetector and light source, respectively.

Kinetics and Mechanism of Metal-Catalyzed Lateral Epitaxy for Growing Lattice-Mismatched Heterostructures via Vapor-Liquid-Solid

Abstract Body: Conductors having at least one dimension at the nanoscale have properties that differ substantially from their bulk counterparts. In particular, electrical resistivity increases significantly when size is reduced while thermal conductivity (κ) decreases. These factors present a critical technological barrier to miniaturization, since the former increases self-heating when current is driven while the latter limits dissipation of that heat from device-active regions. Despite the prominent role of metallic nanostructures in current and future electronics and photonics, large gaps exist in understanding the influence of “size effects” on thermal characteristics at small dimensions. In particular, there is a paucity of direct measurements of thermal conductivity for technologically-relevant materials. This study focuses on development and test of a method for directly measuring κ for conducting nanofilms and nanowires. We report on design, fabrication, test, and application of this approach to 50 and 100 nm thick evaporated gold structures with lateral dimensions ranging from 74 to 720 nm, thereby spanning the nano- to meso-scale. Measurements are carried out at ambient room and 100° C temperatures, i.e., in the standard operating range of low-power electronics. A decrease in κ is observed as gold thickness is reduced. At large lateral width, corresponding to the microscale and analogous to thin films, κ values are found to be 200 and 280 W/mK for thicknesses of 50 and 100 nm, respectively (room temperature). These are to be compared with the accepted value of 317 W/mK for κ of bulk gold. In addition, as the width is reduced, for either thickness, a dramatic decrease in κ is observed beginning at ~ 300 nm width. For the smallest nanowire investigated, 50 nm in thickness and 74 nm in width, a value of κ = 56 W/mK is obtained. At higher test temperature, the thermal conductivities are found to decrease, as expected. The decrease in κ with diminishing size are primarily attributed to grain boundary and surface/interface scattering of electrons—that conduct most of the heat in gold—and quantitatively interpreted using the Boltzmann Transport Equation (BTE).

Direct Measurement of Thermal Conductivity of Gold from Meso- to Nano-Scale

Abstract Body: A material with a high thermoelectric figure of merit plays an important role in the development of efficient thermoelectric devices. Modification of thermal transport in a crystal lattice is one of the most sought-after methods of developing novel thermoelectric materials. Increasing phonon scattering in a crystalline material to lower thermal transport is one way of achieving this objective. A fundamental understanding of the effects of structural features on the thermal properties is a significant first step towards enhanced thermoelectric properties of a material. Although certain quaternary chalcogenides have been examined for their applications as thermoelectric materials, fundamental research into altering the thermal conductivity of this large class of materials remains to be explored. This work contributes towards this area of research by investigating the thermal conductivity and heat capacity of select quaternary chalcogenides to analyze their structure-property relationships. Phenomenological models were utilized to examine the thermal conductivity, κ, and heat capacity, Cp, of BaCu2SnQ4 (Q = S, Se) and BaCdSnSe4. The Debye-Callaway model was employed to investigate the phonon scattering phenomena that occur in these materials. Our analyses indicate similar anharmonicity in all crystal lattices. Furthermore, highly distorted corner-sharing chalcogen tetrahedra encompassing Cu/Cd atoms give rise to large thermal parameters for Cu/Cd in these materials. Relatively high scattering from soft modes in BaCu2SnS2Se2 was identified, such dynamic disorder resulting in very low κ values. Additional disorder for BaCu2SnS2Se2 is due to alloying, causing the lowest κ among the quaternary chalcogenides. The Debye and Einstein temperatures from Cp data corroborated the results obtained from our analyses of the κ data. The large primitive cells with complex lattice vibrations these materials possess lead to an increase in optical modes that further suppress κ. These results and analyses, as well as further recent results on other quaternary chalcogenides, demonstrate the direct impact of complex structural features on phonon dynamics, enhancing our fundamental understanding of the thermal properties of these materials. With material property developments being a significant aspect of thermoelectrics research, our results will aid investigations of other quaternary chalcogenides of interest for thermoelectric applications, as will be described in this presentation.

A Fundamental Study of Structural Effects on Thermal Properties of Quaternary Chalcogenides

Abstract Body: Global fifth-generation (5G) coverage has the potential to underpin the internet-of-things (IoT) ecosystem. Radio frequency (RF) microelectromechanical system (MEMS) filters based on Al1-xScxN are replacing AlN-based devices because of the higher achievable bandwidths. [1] However, overheating of Al1-xScxN film bulk acoustic wave resonators (FBARs) used in RF MEMS filters limits power handling and thus the phone’s ability to operate in an increasingly congested RF environment while maintaining its maximum data transmission rate. Despite this, the factors limiting thermal transport within Al1-xScxN have not been examined. This work investigated the physics that govern the thermal transport within Al1-xScxN, a fundamental building block for 5G RF MEMS. The thermal conductivities of c-axis textured Al1-xScxN films were found to be one order of magnitude lower than similarly textured polycrystalline AlN films and two orders of magnitude lower than single crystal and/or bulk AlN. This abrupt reduction of thermal conductivity with incorporation of Sc atoms into the AlN crystal can be understood in terms of phonon-alloy/disorder scattering, in the context of the phonon gas theory. Increasing the Sc composition results in a further decrease in the thermal conductivity due to structural frustration and lattice softening, which is an effect absent in isomorphs such as Al1-xGaxN. [2] A relatively strong film thickness dependence of the thermal conductivity was observed for the Al1-xScxN films. However, thermal conductivity measurement at varying ambient temperatures exhibited a weak temperature dependence. The impact of abnormally oriented grains on the cross-plane thermal conductivity was found to be negligible for the piezoelectrically functional Al1-xScxN films tested in this work. Outcomes of this work support the electro-thermo-mechanical co-design of 5G Al1-xScxN-based RF acoustic filters. From a thermal standpoint, for Al1-xScxN-based bulk acoustic wave (BAW) filters, the solidly mounted resonator (SAW) configuration would be preferred over the FBAR (free-standing membrane) configuration due to the poor thermal conductivity of Al1-xScxN. The thermal property data set generated in this work reveals design trade-offs for (i) increasing the Sc composition of Al1-xScxN to maximize the electromechanical coupling factor, (ii) decreasing the film thickness to achieve higher GHz-range resonance frequencies, (iii) higher operating temperatures resulting from higher integration density and RF input powers. The thermal conductivity data will allow construction of multi-physics device models that will enable the design and development of Al1-xScxN RF filter technologies with enhanced device performance and improved lifetime. Acknowledgment: This material is based upon work supported by the National Science Foundation, as part of the Center for Dielectrics and Piezoelectrics under Grant Nos. IIP-1361571, IIP-1361503, IIP-1841453, and IIP-1841466. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. G.E. would like to gratefully thank Sara Dickens and Joseph Michael at Sandia for conducting the EBSD analysis. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. DOE’s National Nuclear Security Administration under contract DE-NA-0003525. The views expressed in the article do not necessarily represent the views of the U.S. DOE or the United States Government. References: [1] G. Piazza, V. Felmetsger, P. Muralt, R. H. Olsson III, R. Ruby, MRS Bull. 2012, 37, 1051. [2] K. R. Talley, S. L. Millican, J. Mangum, S. Siol, C. B. Musgrave, B. Gorman, A. M. Holder, A. Zakutayev, G. L. Brennecka, Phys. Rev. Mater. 2018, 2, 63802.

Thermal Conductivity of Al1-xScxN for 5G RF MEMS Filters

Abstract Body: As Moore's Law reaches its natural saturation, it has become crucial to investigate novel devices and materials for high-performance computing. One promising approach is to develop brain-like connected neuromorphic architectures composed of elemental devices capable of non-linear phenomena, such as spiking and potentiation. Much progress towards this end has been made using oxide materials like VO2 and NbO2, in which memristive behavior arises as a consequence of non-linear conductance mechanisms and of the inherent metal-insulator transition (MIT). However, much work remains to be done to correlate device properties, especially performance versus energy cost, to underlying materials properties like effective energy barriers and conductance changes across the MIT. In this work, we investigate these issues by developing a compact model for individual vanadium dioxide devices, so as to link complex dynamic behavior to underlying material and device properties. Using a combination of steady-state current-voltage sweeps, time-varying oscillations, and a novel thermoreflectance temperature-measuring technique, we extract thermal and electrical conductance and capacitance model parameters, and show that the model reproduces all observed device behavior. Finally, we exploit the link between dynamics and materials parameters embodied by the compact model to develop non-trivial device scaling laws, and also experimentally demonstrate a capacitance-controlled bifurcation from stable to unstable oscillating dynamics. This work lays the foundation for future studies allowing disparate memristive materials to be compared through the compact model framework, as well as to begin investigating the even more complex dynamical behaviors arising from couplings of pairs or networks of non-linear devices.

On the Initial Growth Mechanisms of α-Phase Ga2O3 on c-Plane Sapphire by Mist CVD

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On the Initial Growth Mechanisms of α-Phase Ga2O3 on c-Plane Sapphire by Mist CVD

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